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Chem Sci ; 10(2): 564-568, 2019 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-30713652


Controlled trapping atom-precise ultrasmall silver nanoparticles into silver nanoclusters is challenging; thus only limited progress has been made in this area. We are therefore inspired to isolate two novel silver nanoclusters, Ag10@Ag70 (SD/Ag80a and SD/Ag80b; SD = SunDi), where a novel fcc-structured Ag10 kernel built from two single-edge opened Ag6 octahedra by sharing one edge is trapped. The bioctahedral Ag10 kernel is locked by a pair of Mo7O26 10- anions to form an inner Ag10@(Mo7O26)2 core which is further encapsulated by an outer Ag70 shell to form three-shell Ag10@(Mo7O26)2@Ag70 nanoclusters. Notably, the bioctahedral Ag10 kernel has not been observed in silver nanoclusters ever before, thus representing a new embryo state of silver nanoparticles. SD/Ag80a emits in the near infrared (NIR) region (λ em = 730 nm) at low temperature. This work will deepen our understanding on the atomic-level growth of silver nanoparticles and complicated three-shell self-assembly involving polyoxometalate (POM) and two different silver nanoclusters.

Chemistry ; 24(56): 15096-15103, 2018 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-30016561


Introducing phenylphosphonic acid (H2 PPA) into the Ag/tBuSH assembly system has produced a family of nanoscale-sized, high-atom number, silver thiolate/PPA nests (SD/Ag45 a, SD/Ag66 a, and SD/Ag73 a) with impressive core-shell features. SD/Ag45 a is a 45-atom ellipsoid comprised of an Ag36 shell trapping an Ag9 S2 three-bladed rotor inside. SD/Ag66 a comprises an inner rod-like Ag20 core and an outer Ag44 shell, giving a 64-atom nest. These Ag64 nests are further extended by Ag(CN)2 linkers to form a one-dimensional chain structure. SD/Ag73 a is a three-shell 73-nucleus silver nest with a central silver atom enclosed in a rhombicuboctahedron of 24 silver atoms, which is itself enclosed in the outermost shell of a rectified version of a 48-Ag octahedral Goldberg 2,0 cage. The solution behaviors and optical absorption properties of the three nests are described in detail. Of note, SD/Ag45 a and SD/Ag73 a emit in the near-infrared region and show different luminescent thermochromic behavior. This work demonstrates that the participation of H2 PPA strongly influences the structures of silver thiolate nests, thus providing a new route to fabricate and modify them in a more rational way.

Chemistry ; 24(19): 4967-4972, 2018 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-29380899


Compared with the well-known anion-templated effects in shaping silver thiolate clusters, the influence from the organic ligands in the outer shell is still poorly understood. Herein, three new benzoate-functionalized high-nuclearity silver(I) thiolate clusters are isolated and characterized for the first time in the presence of diverse anion templates such as S2- , α-[Mo5 O18 ]6- , and MoO42- . Single-crystal X-ray analysis reveals that the nuclearities of the three silver clusters (SD/Ag28, SD/Ag29, SD/Ag30) vary from 32 to 38 to 78 with co-capped tBuS- and benzoate ligands on the surface. SD/Ag28 is a turtle-like cluster comprising a Ag29 shell caging a Ag3 S3 trigon in the center, whereas SD/Ag29 is a prolate Ag38 sphere templated by the α-[Mo5 O18 ]6- anion. Upon changing from benzoate to methoxyl-substituted benzoate, SD/Ag30 is isolated as a very complicated core-shell spherical cluster composed of a Ag57 shell and a vase-like Ag21 S13 core. Four MoO42- anions are arranged in a supertetrahedron and located in the interstice between the core and shell. Introduction of the bulky benzoate changes elaborately the nuclearity and arrangements of silver polygons on the shell of silver clusters, which is exemplified by comparing SD/Ag28 and a known similar silver thiolate cluster. The three new clusters emit luminescence in the near-infrared (NIR) region and show different thermochromic luminescence properties. This work presents a flexible approach to synthetic studies of high-nuclearity silver clusters decorated by different benzoates, and structural modulations are also achieved.